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Title: Highly mobile charge-transfer excitons in two-dimensional WS2/tetracene heterostructures

Abstract

Charge-transfer (CT) excitons at heterointerfaces play a critical role in light to electricity conversion using organic and nanostructured materials. However, how CT excitons migrate at these interfaces is poorly understood. We investigate the formation and transport of CT excitons in two-dimensional WS2/tetracene van der Waals heterostructures. Electron and hole transfer occurs on the time scale of a few picoseconds, and emission of interlayer CT excitons with a binding energy of ~0.3 eV has been observed. Transport of the CT excitons is directly measured by transient absorption microscopy, revealing coexistence of delocalized and localized states. Trapping-detrapping dynamics between the delocalized and localized states leads to stretched-exponential photoluminescence decay with an average lifetime of ~2 ns. The delocalized CT excitons are remarkably mobile with a diffusion constant of ~1 cm2 s-1. These highly mobile CT excitons could have important implications in achieving efficient charge separation.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Purdue Univ., West Lafayette, IN (United States)
Publication Date:
Research Org.:
Purdue Univ., West Lafayette, IN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1499924
Grant/Contract Number:  
SC0016356
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 4; Journal Issue: 1; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhu, Tong, Yuan, Long, Zhao, Yan, Zhou, Mingwei, Wan, Yan, Mei, Jianguo, and Huang, Libai. Highly mobile charge-transfer excitons in two-dimensional WS2/tetracene heterostructures. United States: N. p., 2018. Web. doi:10.1126/sciadv.aao3104.
Zhu, Tong, Yuan, Long, Zhao, Yan, Zhou, Mingwei, Wan, Yan, Mei, Jianguo, & Huang, Libai. Highly mobile charge-transfer excitons in two-dimensional WS2/tetracene heterostructures. United States. https://doi.org/10.1126/sciadv.aao3104
Zhu, Tong, Yuan, Long, Zhao, Yan, Zhou, Mingwei, Wan, Yan, Mei, Jianguo, and Huang, Libai. Fri . "Highly mobile charge-transfer excitons in two-dimensional WS2/tetracene heterostructures". United States. https://doi.org/10.1126/sciadv.aao3104. https://www.osti.gov/servlets/purl/1499924.
@article{osti_1499924,
title = {Highly mobile charge-transfer excitons in two-dimensional WS2/tetracene heterostructures},
author = {Zhu, Tong and Yuan, Long and Zhao, Yan and Zhou, Mingwei and Wan, Yan and Mei, Jianguo and Huang, Libai},
abstractNote = {Charge-transfer (CT) excitons at heterointerfaces play a critical role in light to electricity conversion using organic and nanostructured materials. However, how CT excitons migrate at these interfaces is poorly understood. We investigate the formation and transport of CT excitons in two-dimensional WS2/tetracene van der Waals heterostructures. Electron and hole transfer occurs on the time scale of a few picoseconds, and emission of interlayer CT excitons with a binding energy of ~0.3 eV has been observed. Transport of the CT excitons is directly measured by transient absorption microscopy, revealing coexistence of delocalized and localized states. Trapping-detrapping dynamics between the delocalized and localized states leads to stretched-exponential photoluminescence decay with an average lifetime of ~2 ns. The delocalized CT excitons are remarkably mobile with a diffusion constant of ~1 cm2 s-1. These highly mobile CT excitons could have important implications in achieving efficient charge separation.},
doi = {10.1126/sciadv.aao3104},
journal = {Science Advances},
number = 1,
volume = 4,
place = {United States},
year = {Fri Jan 12 00:00:00 EST 2018},
month = {Fri Jan 12 00:00:00 EST 2018}
}

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Cited by: 104 works
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Figures / Tables:

Fig. 1. Fig. 1.: Construction of a 1L-WS2/Tc heterostructure. (A) Optical image of WS2 flakes exfoliated on a Si/SiO2 substrate. The 1L-WS2 is indicated by the dashed line. The square shows the area imaged by AFM in (B). Scale bar, 10 mm. (B) AFM image of the same 1L-WS2 flake in (A)more » with a Tc thin film deposited on top. Scale bar, 5 mm. (C) Schematic of the formation of CT excitons and the band alignment of the 1L-WS2/Tc heterostructure, showing the formation of a type II heterojunction. (D) Steady-state PL spectra of a 1L-WS2, Tc thin film, and a 1L-WS2/Tc heterostructure. The new emission band at 1.7 eV indicates the formation of interlayer CT excitons.« less

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